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Electrochemical Reduction of X-ray Contrast Iohexol at Mixed Metal Oxide Electrodes: Process Optimization and By-product Identification

机译:混合金属氧化物电极上X射线对比碘海醇的电化学还原:工艺优化和副产物鉴定

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摘要

The reduction of commonly used X-ray contrast iohexol (IOX) by the electrooxidation process is presented in this study. To begin with, the effect of anode material was examined, and different mixed metal oxide electrodes (MMOs) such as Ti/RuO2, Ti/Pt, Ti/IrO2-RuO2, Ti/IrO2-Ta2O5, Ti/Ta2O5-SnO2-IrO2, and Pt/SnO2 were used. To assess experimental conditions at Ti/RuO2 anode, provided the highest removal efficiency, the response surface method was applied and the key influencing parameter was the process time. The determined optimal conditions were triplicated with real wastewater samples, and the average degradation efficiency of IOX was found to be 99%. By-products of the IOX degradation on the Ti/RuO2 anode have been identified using density functional theory and LC/MS-MS analysis. The results showed that IOX degradation opened with OH group detachment and resulted in the formation of a by-product with a molecular mass of 804 g mol(-1). Further degradation mechanism took place due to the breakup of C-4-C-10 and C-5-I-7 bonds with a by-product formed as 603 g mol(-1). Iodide atom replacement by OH groups caused the formation of a molecular fragment with 375 g mol(-1) molecular weight. The further disintegration of C-2-C-11 and C-6-N-16 sigma- bonds led to the formation of molecular masses of 133, 126, and 119 g mol(-1), respectively.
机译:在这项研究中提出了通过电氧化过程减少常用的X射线对比碘海醇(IOX)。首先,检查阳极材​​料的效果,并使用不同的混合金属氧化物电极(MMO),例如Ti / RuO2,Ti / Pt,Ti / IrO2-RuO2,Ti / IrO2-Ta2O5,Ti / Ta2O5-SnO2-IrO2 ,并使用Pt / SnO2。为了评估在Ti / RuO2阳极上的实验条件(提供最高的去除效率),应用了响应面法,关键的影响参数是工艺时间。将确定的最佳条件与实际废水样品一式三份,发现IOX的平均降解效率为99%。使用密度泛函理论和LC / MS-MS分析,已经确定了Ti / RuO2阳极上IOX降解的副产物。结果表明,IOX降解随OH基团的分离而打开,并导致形成分子量为804 g mol(-1)的副产物。由于C-4-C-10和C-5-I-7键断裂,副产物为603 g mol(-1),形成了进一步的降解机理。碘原子被OH基团取代导致形成分子量为375 g mol(-1)的分子片段。 C-2-C-11和C-6-N-16 sigma-键的进一步分解导致分别形成133、126和119 g mol(-1)的分子量。

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